Journal
ACS CATALYSIS
Volume 6, Issue 9, Pages 6018-6024Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b01429
Keywords
ruthenium; C-60; fulleride; nitrobenzene hydrogenation; amine synthesis
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Funding
- Centre National de la Recherche Scientifique (CNRS)
- China Scholarships Council (CSC)
- Calcul en Midi-Pyrenees initiative-CALMIP [p0812]
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Electron-deficient ruthenium nanoparticles supported on Ru fulleride nanospheres allow the successive and chemoselective hydrogenation of nitrobenzene to aniline and then to cyclohexylamine. The catalysts were prepared in a straightforward manner by decomposition under dihydrogen of [Ru(COD)(COT)] in the presence of C-60. The nitrobenzene hydrogenation reaction is solvent sensitive and proceeds more quickly in methanol than in other alcohols. The same behavior, i.e. a two-step successive hydrogenation, has been observed for several substituted nitroarenes. Density functional theory calculations suggest that the observed chemoselectivity is mainly governed by the presence of surface hydrides on the electron-deficient Ru nanoparticles. At the threshold value of 1.5 H per Ru surface atom, the formation of aniline is favored due to the net preference of the NO2 coordination.
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